title: Partial oxidation of ethane to oxygenates using Fe- and Cu-containing ZSM-5.
abstract: Iron and copper containing ZSM-5 catalysts are effective for the partial oxidation of ethane with hydrogen peroxide giving combined oxygenate selectivities and productivities of up to 95.2% and 65 mol kgcat(-1) h(-1), respectively. High conversion of ethane (ca. 56%) to acetic acid (ca. 70% selectivity) can be observed. Detailed studies of this catalytic system reveal a complex reaction network in which the oxidation of ethane gives a range of C2 oxygenates, with sequential C-C bond cleavage generating C1 products. We demonstrate that ethene is also formed and can be subsequently oxidized. Ethanol can be directly produced from ethane, and does not originate from the decomposition of its corresponding alkylperoxy species, ethyl hydroperoxide. In contrast to our previously proposed mechanism for methane oxidation over similar zeolite catalysts, the mechanism of ethane oxidation involves carbon-based radicals, which lead to the high conversions we observe.
authors.affiliation: Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building Park Place, Cardiff CF103AT, United Kingdom.
authors.forename: Michael M
authors.initials: MM
authors.lastname: Forde
authors.forename: Robert D
authors.initials: RD
authors.lastname: Armstrong
authors.forename: Ceri
authors.initials: C
authors.lastname: Hammond
authors.forename: Qian
authors.initials: Q
authors.lastname: He
authors.forename: Robert L
authors.initials: RL
authors.lastname: Jenkins
authors.forename: Simon A
authors.initials: SA
authors.lastname: Kondrat
authors.forename: Nikolaos
authors.initials: N
authors.lastname: Dimitratos
authors.forename: Jose Antonio
authors.initials: JA
authors.lastname: Lopez-Sanchez
authors.forename: Stuart H
authors.initials: SH
authors.lastname: Taylor
authors.forename: David
authors.initials: D
authors.lastname: Willock
authors.forename: Christopher J
authors.initials: CJ
authors.lastname: Kiely
authors.forename: Graham John
authors.initials: GJ
authors.lastname: Hutchings